Chemical origin of life

  • Article
    | Open Access

    Transfer of scarce phosphate to organic molecules is a significant challenge for prebiotic chemistry. Here authors show a prebiotic physicochemical cycle to activate orthophosphate and via a kinetically stable, thermodynamically activated molecule phosphorylate all of life’s basic building blocks.

    • Oliver R. Maguire
    • , Iris B. A. Smokers
    •  & Wilhelm T. S. Huck
  • Article
    | Open Access

    The “anti-branching rule”, introduced in 1950, excludes branched polyphosphates from biological relevance due to their supposedly rapid hydrolysis. Here, the authors synthesize monodisperse branched polyphosphates and demonstrate their unexpected stability in water, as well as provide evidence for their competence in phosphorylation.

    • Tobias Dürr-Mayer
    • , Danye Qiu
    •  & Henning J. Jessen
  • Article
    | Open Access

    Active coacervate droplets are droplets coupled to a chemical reaction that maintains them out of equilibrium, which can be used to drive active processes, but coacervates are still subject to passive processes that compete with or mask growth. Here, the authors present a nucleotide-based model for active coacervate droplets that form and grow by fuel-driven synthesis of ATP, and, importantly, do not undergo Ostwald ripening.

    • Karina K. Nakashima
    • , Merlijn H. I. van Haren
    •  & Evan Spruijt
  • Article
    | Open Access

    The transition of prebiotic chemistry to present-day chemistry lasted a very long period of time, but the current laboratory investigations of this process are mostly limited to a couple of days. Here, the authors develop a fully automated robotic prebiotic chemist designed for long-term chemical experiments exploring unconstrained multicomponent reactions, which can run autonomously and uses simple chemical inputs.

    • Silke Asche
    • , Geoffrey J. T. Cooper
    •  & Leroy Cronin
  • Article
    | Open Access

    Evolution selects for the fittest but must operate within the realm of the physically possible. Here, the authors present a theoretical framework that allows them to explore how ten abiotic constraints can shape the operation, regulation, and adaptation of metabolism in E. coli.

    • Amir Akbari
    • , James T. Yurkovich
    •  & Bernhard O. Palsson
  • Article
    | Open Access

    The search for life in the universe is difficult due to issues with defining signatures of living systems. Here, the authors present an approach based on the molecular assembly number and tandem mass spectrometry that allows identification of molecules produced by biological systems, and use it to identify biosignatures from a range of samples, including ones from outer space.

    • Stuart M. Marshall
    • , Cole Mathis
    •  & Leroy Cronin
  • Article
    | Open Access

    UV-induced photodamage that likely occurred during the prebiotic synthesis of DNA and RNA is still an untackled issue for their origin on early Earth. Here, the authors show that substitution of 2,6-diaminopurine for adenine enables repair of cyclobutane pyrimidine dimers with high yields, and demonstrate that both 2,6-diaminopurine and adenine nucleosides can be formed under the same prebiotic conditions.

    • Rafał Szabla
    • , Magdalena Zdrowowicz
    •  & Janusz Rak
  • Article
    | Open Access

    So far, only a few chemical oscillators based on organic reactions have been developed. Here, the authors report both autocatalytic and oscillatory reaction networks that form substituted guanidines from thiouronium salts; when coupled to cascade cyclization, this reaction network produces oscillations in the production of pyrimidine-based heterocycles.

    • Alexander I. Novichkov
    • , Anton I. Hanopolskyi
    •  & Sergey N. Semenov
  • Article
    | Open Access

    Artificial molecular systems can show complex kinetics of reproduction, however their integration into larger ensembles remains a challenge towards evolving higher order functionality. Here authors use show that self-reproducing lipids can initiate and accelerate octanol droplet movement and that reciprocally chemotactic movement of these droplets increases the rate of lipid reproduction substantially.

    • Dhanya Babu
    • , Robert J. H. Scanes
    •  & Nathalie Katsonis
  • Article
    | Open Access

    Furanose species have a key role in the chemistry of life despite their instability over pyranose ones. The authors, through NMR characterization of the anomeric ratios at equilibrium and a non-equilibrium theoretical treatment, show that a steady temperature gradient, at temperatures relevant to the early Earth, favors furanose over pyranose isomers.

    • Avinash Vicholous Dass
    • , Thomas Georgelin
    •  & Francesco Piazza
  • Article
    | Open Access

    Autocatalytic networks may have started evolution during the origin of life. Here, the authors establish a landscape of thousands of RNA networks by barcoded sequencing and microfluidics, and derive relationships between topology and Darwinian properties such as variation and differential reproduction.

    • Sandeep Ameta
    • , Simon Arsène
    •  & Philippe Nghe
  • Article
    | Open Access

    A world preceding the prebiotic RNA-world may have been based on xeno nucleic acids (XNAs), but their replication likely did not require enzymes. Here, the authors demonstrate template-directed non-enzymatic synthesis of an XNA, acyclic l-threoninol nucleic acid, via chemical ligation mediated by N-cyanoimidazole, and achieve a pseudo-primer extension of this XNA with all four nucleobases.

    • Keiji Murayama
    • , Hikari Okita
    •  & Hiroyuki Asanuma
  • Article
    | Open Access

    Mimicking the crowded cytosol of cells in synthetic cells has been a major limitation to the functionality. Here, the authors used the interaction between nickel, nitrilotriacetic acid and histidine tagged proteins to control loading of macromolecules into spatially programmed coacervate-based protocells.

    • Wiggert J. Altenburg
    • , N. Amy Yewdall
    •  & Jan C. M. van Hest
  • Article
    | Open Access

    Photosynthetic formation of manganese (Mn) oxides from dissolved Mn ions was proposed to occur in ancestral photosystems before oxygenic photosynthesis evolved. Here, the authors provide evidence for this hypothesis by showing that photosystem II devoid of the Mn cluster oxidises Mn ions leading to formation of Mn-oxide nanoparticles.

    • Petko Chernev
    • , Sophie Fischer
    •  & Holger Dau
  • Article
    | Open Access

    Short cationic peptides and nucleotides can form complex coacervates, but the influence of reduced multivalency on coacervate functionality was not investigated. Here, the authors report that coacervates formed from short polyions generate distinct pH microenvironments, accumulate RNA and preserve nucleic acid duplexes more efficiently than their longer counterparts.

    • Fatma Pir Cakmak
    • , Saehyun Choi
    •  & Christine D. Keating
  • Article
    | Open Access

    Wet-dry cycling is thought to have enabled the production of molecular building blocks of life. Here, the authors investigate the impact of dehydration/rehydration on RNA-containing complex coacervates, which are membraneless compartments formed by phase separation of polyelectrolyte solutions.

    • Hadi M. Fares
    • , Alexander E. Marras
    •  & Christine D. Keating
  • Article
    | Open Access

    Membraneless organelles are liquid-liquid phase-separated droplets whose behaviour can be regulated by chemical reactions, but this process is poorly understood. Here, the authors report model membraneless organelles based on coacervate droplets that show fuel-driven dynamic behaviour and concentrate functional RNA.

    • Carsten Donau
    • , Fabian Späth
    •  & Job Boekhoven
  • Article
    | Open Access

    ATP acts as a co-substrate in enzyme catalysed reactions, but can also specifically bind metal ions. Here, the authors show that ATP interacts with copper ions and forms a Cu(II)-ATP complex that efficiently catalyses Diels-Alder reactions, and determine ATP residues that are essential for this activity.

    • Changhao Wang
    • , Qianqian Qi
    •  & Jörg S. Hartig
  • Article
    | Open Access

    The feasibility of molecular assemblers as a device to control chemical reactions by positioning molecules with atomic precision is a matter of debate in the literature. Here the authors describe of a rudimentary synthetic molecular assembler, supramolecular aggregate of bifunctional surfactants produced by the reaction of two phase-separated reactants that produces polymers.

    • Anthonius H. J. Engwerda
    •  & Stephen P. Fletcher
  • Article
    | Open Access

    Formation of peptide bonds in cold gas-phase environments might represent a prebiotic synthesis route of polypeptides. Here, the authors show the formation of up to tetra-peptide species in the collision of He2+ ions, with kinetic energies typical for solar wind ions, with cold β-alanine clusters.

    • Patrick Rousseau
    • , Dariusz G. Piekarski
    •  & Bernd A. Huber
  • Article
    | Open Access

    Structurally divergent reactions on racemic mixtures, which produce distinct chemical species from an enantiomeric mixture, are extremely rare in the literature. Here, the authors are able to use a dynamic combinatorial approach to yield structurally divergent, non-isomeric [2]catenanes from an enantiomeric mixture.

    • Tiberiu-M. Gianga
    •  & G. Dan Pantoș
  • Article
    | Open Access

    Cooperative relationships are widespread among different classes of biopolymers and are predicted to have existed during emergence of life. This study shows that proto-peptides engage in mutually stabilizing interactions with RNA, providing support for the co-evolution of these molecules.

    • Moran Frenkel-Pinter
    • , Jay W. Haynes
    •  & Luke J. Leman
  • Article
    | Open Access

    Models of the origin of life generally require a mechanism to structure emerging populations. Here, Krieger et al. develop spatial models showing that coherent structures arising in turbulent flows in aquatic environments could have provided compartments that facilitated the origin of life.

    • Madison S. Krieger
    • , Sam Sinai
    •  & Martin A. Nowak
  • Article
    | Open Access

    The principles of intercellular communication in multicellular organisms can be explored using artificial cells. Here, the authors report on giant vesicles which can recognize diffused chemical signals and amplify the signal by synthetic enzymatic cascades to allow signal propagation over long distances.

    • Bastiaan C. Buddingh’
    • , Janneke Elzinga
    •  & Jan C. M. van Hest
  • Article
    | Open Access

    Selection in compartmentalized self-replicating systems might provide a way for life to arise from abiotic environments. Here, the authors explore selection in a system of transient autocatalytic lipids and find that autocatalytic kinetics and phase separation are the key selection factors.

    • Ignacio Colomer
    • , Arseni Borissov
    •  & Stephen P. Fletcher
  • Article
    | Open Access

    Although bistability is common in biology, it is very difficult to design de novo into synthetic systems. Here, the authors present an experimental and theoretical analysis of a chemical network that displays bistable behavior under certain far-from-equilibrium conditions, and map the parameter space in which bistability operates.

    • Indrajit Maity
    • , Nathaniel Wagner
    •  & Gonen Ashkenasy
  • Article
    | Open Access

    Wet–dry cycling is regarded as a possible driving force of condensation reactions under prebiotic conditions. Here, the authors propose that water uptake by deliquescent minerals could have facilitated the wet phase and simulate this scenario using the oligomerization of glycine as a model reaction.

    • Thomas D. Campbell
    • , Rio Febrian
    •  & Paul J. Bracher
  • Article
    | Open Access

    Cyanide is thought to be crucial for the origin of life. Here, the authors showed that iron cyanocarbonyl complexes are present in meteorites and propose that these compounds were a source of free cyanide on early Earth and served as precursors to the active sites of ancient hydrogenases.

    • Karen E. Smith
    • , Christopher H. House
    •  & Michael P. Callahan
  • Article
    | Open Access

    Understanding how simple chemical mixtures transition into truly emergent systems is essential to create new lifelike materials. Here, the authors show a self-replicating system that can be maintained out-of-equilibrium by an oxidant fuel in analogy to simple metabolic cycles.

    • Sarah M. Morrow
    • , Ignacio Colomer
    •  & Stephen P. Fletcher
  • Article
    | Open Access

    Extraterrestrial sources may have provided prebiotic phosphorus to the early Earth. Here, the authors investigate the potential of phosphine-doped astrochemical analog ices to form phosphorus oxoacids as precursors to more complex prebiotic compounds.

    • Andrew M. Turner
    • , Alexandre Bergantini
    •  & Ralf I. Kaiser
  • Article
    | Open Access

    So far little is known about how encapsulation affects the activity and folding of RNA, which is of interest for understanding the origin of cellular life. Here the authors show that encapsulation of functional RNA in vesicles increases RNA activity and improves RNA folding through a biophysical confinement effect.

    • Ranajay Saha
    • , Samuel Verbanic
    •  & Irene A. Chen
  • Article
    | Open Access

    Understanding self-replication and persistence in an out-of-equilibrium state is key to designing systems with new properties mimicking “living systems”. Here, the authors developed a synthetic small molecule system in which a transient surfactant replicator is responsible for both an autocatalytic aggregation pathway and a destructive pathway.

    • Ignacio Colomer
    • , Sarah M. Morrow
    •  & Stephen P. Fletcher
  • Article
    | Open Access

    There is still much debate on early Earth geochemical conditions affecting the chemistry of simple synthons that originated life. Here, the authors report an uninterrupted multistep synthetic route to 2-aminooxazole by means of flow chemistry equipment, mimicking a plausible early Earth (geo)chemical scenario.

    • Dougal J. Ritson
    • , Claudio Battilocchio
    •  & John D. Sutherland
  • Article
    | Open Access

    Phosphorus is presumed to have been a limiting nutrient in the Archean ocean due to binding to iron oxides. Here, the authors show the heating of iron with phosphate results in the reduction of phosphate to the ion phosphite, which is solubilized and ameliorates the issue of a low Archean phosphorus supply.

    • Barry Herschy
    • , Sae Jung Chang
    •  & Matthew A. Pasek
  • Article
    | Open Access

    Amyloids may have played an important role in prebiotic molecular evolution but understanding replication of such information-coding molecules is still a problem. Here the authors design a model amyloid substrate and demonstrate sequence regio- and stereoselectivity during template-based replication.

    • Saroj K. Rout
    • , Michael P. Friedmann
    •  & Jason Greenwald
  • Article
    | Open Access

    How RNA building blocks have formed on an early Earth by a continuous process is still a mystery awaiting its solution. Here, the authors report that fluctuations of physical parameters like temperature and pH could have been enough to facilitate nucleoside formation from simple starting materials.

    • Sidney Becker
    • , Christina Schneider
    •  & Thomas Carell
  • Article
    | Open Access

    The citric acid cycle (TCA) is a fundamental metabolic pathway to release stored energy in living organisms. Here, the authors report two linked cycles of reactions that each oxidize glyoxylate into CO2 and generate intermediates shared with the modern TCA cycle, shedding light into a plausible TCA protometabolism.

    • Greg Springsteen
    • , Jayasudhan Reddy Yerabolu
    •  & Ramanarayanan Krishnamurthy
  • Article
    | Open Access

    Clay is thought to have played a part in the origin of life. Here, the authors show that layered double hydroxides, a type of clay little studied despite its presumed prevalence on the early Earth, can facilitate the formation of small proteins.

    • Valentina Erastova
    • , Matteo T. Degiacomi
    •  & H. Chris Greenwell
  • Article
    | Open Access

    Proton motive forces are central for life but it is not well understood how these pH gradients emerged at the beginning of life. Here the authors show that heat flow across a water-filled chamber forms and sustains stable pH gradients and support their experimental findings with simulations.

    • Lorenz M. R. Keil
    • , Friederike M. Möller
    •  & Christof B. Mast
  • Article
    | Open Access

    Few studies have explored the effect of a changing environment on artificial chemical evolution. Here, the authors develop an evolutionary platform that alters the physical environment of droplet protocells, showing that a population of simple chemical species can adapt to its surroundings, in analogy to natural evolution.

    • Juan Manuel Parrilla-Gutierrez
    • , Soichiro Tsuda
    •  & Leroy Cronin
  • Article
    | Open Access

    The synthesis of biopolymers in living cells is perfected by complex machinery, however this was not the case on early Earth. Here the authors show the role of non-enzymatic replication in the enrichment of certain products within prebiotically relevant mixtures.

    • Jayanta Nanda
    • , Boris Rubinov
    •  & Gonen Ashkenasy
  • Article
    | Open Access

    Early molecules of life likely served both as templates and catalysts, raising the question of how functionally distinct genomes and enzymes arose. Here, the authors show that conflict between evolution at the molecular and cellular levels can drive functional differentiation of the two strands of self-replicating molecules and lead to copy number differences between the two.

    • Nobuto Takeuchi
    • , Paulien Hogeweg
    •  & Kunihiko Kaneko
  • Article
    | Open Access

    Coupling compartmentalisation and molecular replication is essential for the development of evolving chemical systems. Here the authors show an oil-in-water droplet containing a self-replicating amphiphilic imine that can undergo repeated droplet division.

    • J. W. Taylor
    • , S. A. Eghtesadi
    •  & L. Cronin
  • Article
    | Open Access

    The emergence of novel catalytic functions in ancient proteins likely played a role in the evolution of modern enzymes. Here, the authors use protein sequences from Precambrian beta-lactamases and demonstrate that a single hydrophobic-to-ionizable amino acid mutation can lead to substantial Kemp eliminase activity.

    • Valeria A. Risso
    • , Sergio Martinez-Rodriguez
    •  & Jose M. Sanchez-Ruiz
  • Article
    | Open Access

    While mechanisms have been proposed for the prebiotic nucleotide synthesis, these require separate (and potentially incompatible) routes for pyrimidines and purines. Here the authors show that both of these classes of molecules can be formed by a divergent synthesis from a common prebiotic precursor.

    • Shaun Stairs
    • , Arif Nikmal
    •  & Matthew W. Powner
  • Article
    | Open Access

    Some of the earliest life on Earth flourished in terrestrial hot springs. Here, the authors present evidence for ca. 3.5 Ga hot spring deposits from the Dresser Formation, Pilbara Craton, Australia, that host some of the earliest known life in the form of stromatolites and other microbial biosignatures.

    • Tara Djokic
    • , Martin J. Van Kranendonk
    •  & Colin R. Ward
  • Article
    | Open Access

    Adverse early life experiences can have negative consequences for health and survival in later life. Here, Tung et al. show that in female baboons, the cumulative number of adverse experiences can be a strong predictor of lifespan.

    • Jenny Tung
    • , Elizabeth A. Archie
    •  & Susan C. Alberts